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  • Chenlong Wang, Wanting Hu, Liandi Guan, Xiaoping Yang, Qionglin Liang
    Chinese Chemical Letters. 2022, 33(6): 2883-2892.

    Metabolites can directly reflect and modulate cell responses and phenotypical changes by influencing energy balances, intercellular signals, and many other cellular functions throughout the lifespan of cells. Taking into account the heterogeneity of cells, single-cell metabolite analysis offers an insight into the functional process within one cell. Microfluidics as a powerful tool has attracted significant interest in the single-cell metabolite analysis field. The microfluidic platform is possible to observe, classify, and stimulate individual cells. It can also transport single-cell to subsequent analysis steps in a fast and controllable way to determine and analyze the composition and content of metabolites. The reviews of topics in microfluidics for single-cell metabolite analysis have been published in the past few years. However, most of them focused on metabolite analysis with mass spectrometry. Here, we covered the advances of microfluidic devices for single-cell metabolite analysis, with a focus on single-cell isolation and manipulation. What is more, we summarized the detection methods and applications of single-cell metabolites.

  • Ziai Zhong, Lisha Chen, Longshuai Zhang, Feiyao Wu, Xunheng Jiang, Haiyan Liu, Fengrong Lv, Haiyang Xie, Fanqi Meng, Lingling Zheng, Jianping Zou
    Chinese Chemical Letters. 2022, 33(6): 3061-3064.

    Owing to the exorbitant overpotential and serious carrier recombination of graphitic carbon nitride (g-C3N4), noble metal (NM) is usually served as the H2 evolution co-catalyst. Although the NM (such as Pt) nanoparticles can reduce the H2 evolution overpotential, the weak van der Waals interaction between Pt and g-C3N4 makes against the charge transfer. Herein, the solvothermal method is developed to achieve semi-chemical interaction between Pt and g-C3N4 nanotube (Pt-CNNT) for fast charge transfer. Moreover, the generated in-plane homojunction of CNNT can accelerate charge separation and restrain recombination. Meanwhile, the metallic Pt is an excellent H2 evolution co-catalyst. Photo/electrochemical tests verify that the semi-chemical interaction can improve photogenerated charge separation and transferability of CNNT. As a result, the photocatalytic H2 evolution turnover frequency (TOF) of Pt-CNNT under visible light irradiation reaches up to 918 h−1, which is one of the highest in the g-C3N4-based photocatalysts. This work provides a new idea to improve the charge transfer for efficient photocatalytic H2 evolution.

  • Yuqiang Hu, Zhen Zhang, Wei Zhang, Minghao Hu, Xianjin Xiao, Tongbo Wu
    Chinese Chemical Letters. 2022, 33(6): 3026-3030.

    DNA-functionalized gold nanoparticles are one of the most versatile bionanomaterials for biomedical and clinical diagnosis. Herein, we discovered that the performance of DNAzyme cleaving the substrate is highly related to its length. This intriguing phenomenon only appears at the interfaces of DNA-functionalized gold nanoparticles. We systematically investigated the causes of this phenomenon. We conjectured that the DNAzyme with extended nucleotides that do not match its substrate strand is vulnerable to non-specific adsorption, electrostatic repulsion, and steric hindrance. Based on our improved understanding of this phenomenon, we have successfully developed a highly sensitive and specific amplifiable biosensor to detect human apurinic/apyrimidinic endonuclease 1.

  • Honglan Wang, Yuefei Zhu, Longlong Zhang, Huiwen Liu, Chunying Liu, Bo Zhang, Yanan Song, Yu Hu, Zhiqing Pang
    Chinese Chemical Letters. 2022, 33(6): 2937-2941.

    Uncontrollable hemorrhage remains staple trouble in surgical procedures and a leading cause after major trauma. The bleeding issue may trigger various pathologic scenarios that can lead to tissue morbidities and mortalities, and currently available on-site hemostatic agents are confined to a narrow therapeutic index and may carry the risk of immunogenicity. Inspired by the crucial role of platelets in the process of thrombus, a platelet-mimetic plateletsome with wound targeting and blood coagulation properties is developed for hemorrhage control. Plateletsome is formulated by integrating platelet membranes with functionalized synthetic liposomes and exhibits superior wound targeting and effective hemostasis properties. It presents less blood loss and shorter hemostasis time than the platelet membrane vehicles or the conventional liposomes in the mouse tail transection model. The strong homing of the biomimetic plateletsome to the thrombus was also confirmed, demonstrating the potential of this engineered cell membrane vesicle as a biomimetic hemostat for bleeding treatment.

  • Jingjing Yan, Ling Miao, Hui Duan, Dazhang Zhu, Yaokang Lv, Liangchun Li, Lihua Gan, Mingxian Liu
    Chinese Chemical Letters. 2022, 33(5): 2681-2686.

    A facile fabrication strategy is reported to obtain N/O codoped porous carbon nanosheets for purpose of ameliorating the charge transfer and accumulation in the concentrated LiTFSI (lithium bis(trifluoromethane sulfonyl)imide) electrolyte. By tunning the feed ratio of comonomers, the porous nanosheet structure is endowed with a significant ion-adsorption surface area (1630 m2/g) and interconnected hierarchical porosity; meanwhile, high-level N/O dopants (N: 3.58 at%, O: 12.91 at%) increase the effective contact area for electrolyte ions, and further facilitate rapid ion/electron transfer. Benefiting from the advantageous features, carbon nanosheets electrode reveal an enhanced specific capacitance (375 F/g) in three-electrode configuration and the H2SO4-based device yields a high gravimetric energy density of 11.4 Wh/kg. Particularly, the ion-diffusion highways in porous carbon nanosheets contribute to the 2.25 V LiTFSI-based symmetric device with a high energy delivery up to 33.1 Wh/kg. This work offers an inspiring strategy for facile fabrication of carbon nanosheets, and demonstrates their promising application in "water-in-salt" electrolyte-based supercapacitor systems.

  • Lijuan Xu, Ye Tu, Jiao Li, Wannian Zhang, Zhibin Wang, Chunlin Zhuang, Lei Xue
    Chinese Chemical Letters. 2022, 33(5): 2545-2549.

    Targeting RIPK1 is a promising strategy for the treatment or alleviation of acute lung injury (ALI). SZM594, a benzothiazole compound previously developed by our research group, possessed good dual-targeting receptor-interacting protein kinase 1 (RIPK1) and RIPK3 activity and anti-necroptosis activity as well as acceptable in vivo efficacy. In this study, the cyclopropyl moiety of SZM594 was modified based on a structure-based design strategy. The resulting cyclohexanone-containing analogue 41 improved the selectivity toward RIPK1 over RIPK3 and the anti-necroptosis activity was also increased compared with those of SZM594. More importantly, compound 41 could inhibit the tumor necrosis factor-α (TNF-α) expression in lipopolysaccharide (LPS)-induced peritoneal macrophage cell model, and significantly alleviate LPS-induced ALI in a mouse model. This compound could significantly inhibit the expressions of the phosphorylation of RIPK1 and down-stream RIPK3 and mixed lineage kinase domain-like protein (MLKL). Thus, these cyclohexanone-containing benzothiazole analogues represent promising lead structures for the discovery of novel protective agents of ALI.

  • Zefeng Gu, Anchen Fu, Ru Qiu, Ru Sun, Zhijuan Cao
    Chinese Chemical Letters. 2022, 33(5): 2711-2714.

    DNA-based logic gates promote the development of molecular computing and show enormous potential in the fields of nanotechnology and biotechnology. Dumbbell oligonucleotides (DNA) with poly-thymine (poly-T) loops and a nicked random double strand have been demonstrated to be an efficient template for the formation of fluorescent copper nanoclusters (CuNCs) in our previous work. Herein, a new platform technology is presented with which to construct molecular logic gates by employing CuNCs probe as a basic output generator, coupling of functional nucleases as the inputs. Two dumbbell DNAs are used with the difference in stem length (8 bp and 16 bp, respectively). The degradation of DNA templates can be tuned by various nucleic acid enzymes, single-stranded nuclease (S1), double-stranded specific nuclease (DSN), E. coli DNA ligase, exonucleases Ⅰ and Ⅲ. Briefly, S1 can digest both DNA templates, while the cleavage ability of DSN will be resistant by the short stem of SS-DNA (short-stem DNA). Exonuclease Ⅰ and Ⅲ can degrade these two nicked DNA templates, which are inhibited due to the ligation of E. coli DNA ligase. With this novel strategy, a set of logic gates is successfully constructed at the molecular level, including "YES", "PASS 0", "OR", "INHIBIT", which take the advantages of no label, easy operation, fast speed, high efficiency and low cost. Furthermore, S1 nuclease, as the biomarker of numerous carcinogens, is selectively detected in the range of 0.05–50 U/mL with the detection limit of 0.005 U/mL (1 × 10−6 U) based on this platform.

  • Lin Wang, Xinzhe Li, Chengjie Pei, Cong Wei, Jie Dai, Xiao Huang, Hai Li
    Chinese Chemical Letters. 2022, 33(5): 2611-2616.

    The properties of two-dimensional (2D) materials are highly dependent on their phase and thickness. Various phases exist in tin disulfide (SnS2), resulting in promising electronic and optical properties. Hence, accurately identifying the phase and thickness of SnS2 nanosheets is prior to their optoelectronic applications. Herein, layered 2H-SnS2 and 4H-SnS2 crystals were grown by chemical vapor transportation and the crystalline phase of SnS2 was characterized by X-ray diffraction, ultralow frequency (ULF) Raman spectroscopy and high-resolution transmission electron microscope. As-grown crystals were mechanically exfoliated to single- and few-layer nanosheets, which were investigated by optical microscopy, atomic force microscopy and ULF Raman spectroscopy. Although the 2H-SnS2 and 4H-SnS2 nanosheets have similar optical contrast on SiO2/Si substrates, their ULF Raman spectra obviously show different shear and breathing modes, which are highly dependent on their phases and thicknesses. Interestingly, the SnS2 nanosheets have shown phase-dependent electrical properties. The 4H-SnS2 nanosheet shows a current on/off ratio of 2.58 × 105 and excellent photosensitivity, which are much higher than those of the 2H-SnS2 nanosheet. Our work not only offers an accurate method for identifying single- and few-layer SnS2 nanosheets with different phases, but also paves the way for the application of SnS2 nanosheets in high-performance optoelectronic devices.

  • Xiang Chen, Zhihong Zhu, Shanshan Liu, Yi-Hung Chen, Xiao Shen
    Chinese Chemical Letters. 2022, 33(5): 2391-2396.

    Herein, we report an unprecedented regiospecific oxidative Mizoroki-Heck type reaction for the synthesis of α-difluoromethyl homoallylic alcohols. The reaction shows broad substrate scopes and high functional group tolerance. Late-stage functionalization of complex biologically active molecules demonstrates the synthetic potential of this transformation. Mechanistic study supports the involvement of MnBr2 catalyzed radical 1, 2-silyl transfer.

  • Menghui Xi, Chaozheng He, Houyong Yang, Xi Fu, Ling Fu, Xiaoli Cheng, Jiyuan Guo
    Chinese Chemical Letters. 2022, 33(5): 2595-2599.

    We predicted two stable two-dimensional materials of carbon and bismuth elements, namely BiC and Bi2C monolayers. The stabilities of two monolayers were examined by cohesive energy, Born criteria, first-principle MD simulations and phonon spectra, respectively. By including the spin-orbit coupling effects, the BiC monolayer is a metal and the Bi2C monolayer possesses a narrow direct (indirect) band gap of 0.403 (0.126) eV under the HSE06 (GGA-PBE) functional. For the adsorption of CO2 molecules, the BiC and Bi2C monolayers have three stable adsorption sites C2, T3 and T4 with the adsorption energies as -0.57, -0.51 and -0.81 eV, and the activation ability on the adsorption as T4 > T3 > C2. These consequences make the BiC and Bi2C monolayers to be promising adsorbents to capture CO2 gas, the Bi2C monolayer to be well photovoltaics and optoelectronics material, and the BiC monolayer to be ideal battery and electronics materials, respectively.

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